Around the world, renewable energy use including solar, wind, hydro, geothermal, and bio-energy are on the rise, and these alternative sources could hold a key to combating climate change. Solar energy is one of the most promising renewable energy resources which uses the never-ending energy of the sun at least for the next 4.5 billion years. Different types of technologies have been employed to harness the immense solar energy potential. In this study, natural dye-sensitized solar cells (DSSCs) were investigated through experimental and computational methods. Different types of organic dyes extracted from selected plant species were investigated. A mixture of solvents (ethanol, methanol, and tetrahydrofuran (THF)) with a ratio of 1:1:1 was used to extract organic molecules from these plants. Natural dye sensitizers were extracted from the petals of Gazania rigens, Pelargonium zonale, Euryops pectinatus, Cestrum elegance, Campsis radicans, and Euphorbia pulcherrima. The optical characteristics of the sensitizers were measured using a UV-Vis spectrophotometer, and all sensitizers showed an absorption range from near UV to visible regions. All calculations presented in this study were performed using density functional theory (DFT) implemented in the Gaussian 09W software. The B3LYP and a basis set of 6-31G++, (d, p) level of theory were chosen to optimize the geometries and energetics of dye molecules. The bandgap of the molecules was obtained from the highest occupied molecular orbital (HOMO) and lower unoccupied molecular orbital (LUMO). Results revealed a bandgap of the dye molecules are in the range of 2.16 - 2.38eV and the bandgap of pristine TiO2 is (3.2 eV). DSSCs are fabricated from the photoanode (FTO glass coated with T/SP and R/SP) and counter-electrode (FTO coated with graphite) in the presence of I-/I3- electrolyte. The photochemical performances of various DSSCs based fabricated devices were evaluated and among all examined sensitizers, Euryops pectinatus sensitizer shows the highest efficiency of 1.03%.